Dynamic Phase Diagram of Catalytic Surface of Hexagonal Boron Nitride under Conditions of Oxidative Dehydrogenation of Propane

Zhang, Zisheng1,2; Jimenez-Izal, Elisa1,3,4; Hermans, Ive5; Alexandrova, Anastassia N.1,6

2019-01-03

10.1021/acs.jpclett.8b03373

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

Partially oxidized surfaces of hexagonal boron nitride (hBN) and several metal borides are unexpectedly excellent catalysts for oxidative dehydrogenation of alkanes to olefins, but the nature of the active site(s) on these B-containing interfaces remains elusive. We characterize the surface of the partially oxidized B-rich hBN surface under reaction conditions from first principles. The interface has thermal access to multiple different stoichiometries and multiple structures of each stoichiometry. The size of the thermal ensemble is composition-dependent. The phase diagram of the interface constructed on the basis of the statistical ensembles of many accessible states is very different from the one based on global minima. Phase boundaries shift and blur, and phases consist of several stoichiometries and structures. The BO layer transiently exposes the reactive -B=0 motifs in the metastable states. The fluxionality and structural diversity emerging under reaction conditions must be taken into account in theoretically descriptions of the catalytic interface.

SCI ; EI

英语

NI论文

其他

Postdoctoral Fellowship of the Basque Country[POS 2015 1 0008]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000455168800004

AMER CHEMICAL SOC

20190206359974

Boron nitride ; Catalyst activity ; Dehydrogenation ; III-V semiconductors ; Nitrides ; Phase diagrams ; Stoichiometry ; Surface reactions

Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Classical Physics; Quantum Theory; Relativity:931 ; High Energy Physics; Nuclear Physics; Plasma Physics:932

Web of Science

1.Univ Calif Los Angeles, Dept Chem & Biochem, 607 Charles E Young Dr, Los Angeles, CA 90095 USA
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
3.Euskal Herriko Unibertsitatea, Kim Fak, UPV EHU, PK 1072, Donostia San Sebastian 20080, Euskadi, Spain
4.DIPC, PK 1072, Donostia San Sebastian 20080, Euskadi, Spain
5.Univ Wisconsin, Dept Chem, 1101 Univ Ave, Madison, WI 53706 USA
6.Calif NanoSyst Inst, Los Angeles, CA 90095 USA

Zhang, Zisheng,Jimenez-Izal, Elisa,Hermans, Ive,et al. Dynamic Phase Diagram of Catalytic Surface of Hexagonal Boron Nitride under Conditions of Oxidative Dehydrogenation of Propane[J]. Journal of Physical Chemistry Letters,2019,10(1):20-25.

Zhang, Zisheng,Jimenez-Izal, Elisa,Hermans, Ive,&Alexandrova, Anastassia N..(2019).Dynamic Phase Diagram of Catalytic Surface of Hexagonal Boron Nitride under Conditions of Oxidative Dehydrogenation of Propane.Journal of Physical Chemistry Letters,10(1),20-25.

Zhang, Zisheng,et al."Dynamic Phase Diagram of Catalytic Surface of Hexagonal Boron Nitride under Conditions of Oxidative Dehydrogenation of Propane".Journal of Physical Chemistry Letters 10.1(2019):20-25.